Scalable and Sustainable Cathode Regeneration from Blended Spent Batteries into Stable Lithium-Rich Manganese-Based Cathodes

Graphical This study presents a scalable cathode recycling method using a continuous stirred-tank reactor to produce high-performance Li-rich Mn-based cathodes, which achieves 97.38% metal recovery rate and over 500 cycles of superior cycling stability, 22.74% longer lifespan than commercial materials. Life-cycle and economic analyses indicate a 44.22% reduction in costs and significant ecobenefits across all midpoint and endpoint impact categories. As a vital urban mineral resource, the efficient recycling of spent lithium-ion batteries (LIBs) is crucial for mitigating resource scarcity and environmental pollution, especially for obtaining high-value cathode materials through various regeneration methods. Herein, a large-scale recyclable and sustainable direct cathode regeneration strategy is explored to obtain stable lithium-rich manganese-based cathode materials via a customized continuous stirred tank reactor, enabling the transition to next-generation high-energy-density LIBs via battery recycling. A high recycling efficiency between 97.38% and 99.93% is achieved for high-value transition metal elements, and the regenerated next-generation higher-specific capacity cathode materials with higher lattice oxygen and lower oxygen vacancy demonstrate better structural stability and improved electrochemical performance than corresponding commercial materials. Life cycle and technoeconomic analysis are used to highlight the cathode regeneration method, which exhibits significant advantages across all 18 midpoint and 3 endpoint environmental impact categories, with a 44.22% cost reduction compared to commercial materials. This commercialization strategy holds significant promise for advancing closed-loop battery recycling and minimizing environmental pollution in LIB production, offering a new perspective for sustainable battery recycling.